Method of making pure unctuous graphite.



UNITED ES i OFFICE.

nnwann eo'omucn Manson, or NIAGARA ramps, onraarjo; cannon.

mentor) 'or MAKING roar. une'ruous GRAPHITE.

No Drawing.

and graphite articles wherein a carbonaceous mass or article capable of transformabody, tion at high temperatures into graphite is electrically heated while protected from the oxidizing action of the air by a covering or envelop of granular or pervious material, which must be of relatively low electrical conductivity as compared with the carbonaceous mass, and refractory to'the extent of remaining pervious to the gases at the highest temperature to which it is subjected. For such envelop I have .heretofore employed a mixture containing sand and caron, this mixture enveloping or covering the carbonaceous mass to be converted into graphite. The enveloping mixture has in practice been relatively shallow, the depth or thickness of the bed or layer being usually approximately one-fourth the diameter of the carbonaceous mass or core to be converted into graphite: furthermore, the sand. and carbon composing the iixture have not been employed in practice 1n pro er proper tions for the formation of carbi of silicon, but in a roportion offering a higher resistance to tie passage of the electric current. Under these conditions, and in the time required tocompletely graphitize the carbonaceous mass or core or the articles contained in or associated therewith, the enveloping mixture is partially converted into carbid of silicon, crystals of which are formed in a thin zone surrounding or partially surrounding the core. The conversion of the mixture into carbid of silicon is however quite incom: plete under the conditions of graph1t1zation,'

and the crystals are never bonded together Into a firm, solid and coherent body, but on the contrary appear in the form of a friable and fragile mass, largely composed of very minute crystals, admixed with unconverted or partially converted material.

In order to recover the graphite from a furnace of this character it is necessary first to remove some portlon of the envelop of sand and carbon, or of sand, carbon and EDWARD Goomncrr of which the fo lowing is a specificationl eating purposes,

Specification of Letters Patent. -Pa,tented Sept, 14,, 1909, Application filed May 10, 1909. Serial No. L157.

carbid'of silicon. It is impossibletoeifect this in practice without breaking the friable mass or detaching considerable quantities of the crystals. These detached portions, cr'ys tals or fragments contaminate the graphite or the outer portions thereof, and

lead to considerable losses and great ex ense, particularly inthe manufacture. o thersoft, unctuous and non-coalescing forms of raphite suitable for lubrication; for it will e evident that a mere trace of the extremely hard and highly abrasive carbid of siliconwill complete y destroy the value of the graphite as a lubricant. For this reason it is customary to carefully remove and reect the portion of the core adjacent the'carid zone, often amounting to200' pounds or more in the charge of a single furnace, and

to carefully separate the carbid of silicon and other foreign matters from the remaining graphiteby concentration in a current of air.

I have now discovered that under proper conditions as hereinafter set forth it 1s possible to so operate the furnace as to obtain in the current path or interior zone of maximum temperature a pure, soft, unctuous and non-coalescing graphite, adapted for lubrior such other grade of graphite or character of graphitearticle as may be desired, in accordance with the materials and arrangement of the core or carbonaceous resister and the time and intensity of heating, and around and enveloping this raphite a shell of carbid of silicon which 1s coherent, firm, self-supporting and -nonfriable in character to such degree that it may be broken up and remove to expose the graphite without seriously contaminating the latter or any portion of it, any detached crystals or crystalline a regates bein of such character as to be readily separated from the graphite. This is not only highly advantageous as regards the yield of graphitefrom the furnaceand the purityof the product, but is also advantageous in that the carbid of silicon so formed is of such character as to be well adapted 'for abrasive purposes, consist-ing, more particularge and well-defined crystals adapted for the manufacture of abrasive wheels. Thus, in addition to its primary functions of preventing combustion 'or oxidation of the graphite and retaining the heat in the furnace while permitting at all stages of the v larly in the portions adjacent the core, of

reaction" a free escape of vapors or gases, it

. constitutes a valuable by-product of the graphite manufacture.

A further advantageflof the process relates to the lncreased purity of the product due to the more complete volatilization of any contained ash or associated non-carbonaceous matters such as sand. I As above pointed out, the product is purer because less subject to contamination from the enveloping material, but it is also inherently =purer because the conditions of theprocess are. such as to bring about the substantially complete elimination of non-carbon constituents. For example,'it has-been found prac ticable to produce a graphite containing from 99.90 to 99.95 per cent. of graphitic carbon,

the residue representing, I believe, only such metallic or other'condensable Va ors as are present in the furnace at the -c ose of the operation 7 and are condensed on cooling upon the surfaces of the gra bite therein. This purity is independent 0 the amount of ash or admixed material originally presentinthe aphite-forming' charge, and I have been a le to obtain'a graphlteof purity. as above indicated from a charge whose .=co'nten't of non-carbonaceous matter. varied from 0.2 per cent. or even less, to 40.0 per cent. or even more of the initial weight of the charge. v

- In order that thepresent invention may be clearly understood, it mafy be ex lamedthat the. initial formation 0 carbi of silicon around a resistance body or core consists of minute crystals which are either separate or,

if aggregated, exist as 'a loose and friable mass. On continued' heating for a suflicient I period the crystals adjacent'the resisterincreasein size, acquire a plate-like form, and

become firmlygbonded or united into a solid and coherent shell. In order however that thisresult may be attained it is necessa This necessity 1s a direct result of the longer not only to continue the heatingffor. amuc longer period than is requisite for the raphitization of the carbonaceous core, but to provide a much deeper or thicker bed or envelop consisting of or containing sand and carbon than is required for the rotection of the core and the conservation -0 the heat when a mere graphitizing effect is sought.

heating period necessary for the rodu'ct on of the firm. and coherent shell 0 carbid of silicon.

It would be quite impossibl'eto obtain a firm or coherent shell of crystals of -the character desired by longerfheating under .the heretofore obtaining conditions in themanufacture of aphite, for the reason that the comparative y thin bed bf'sand and carbon, even though inproper proportions to yield carbid of silicon, would permit too free escape of heat to render'it practicable to maintain the desired temperature for the.

the thickness of the bed or envelo necessary time. A firm and coherent shell can, I believe, be obtained only by providin a much thicker bed or envelo consisting 0 or containing sand and car on, in proportions or the production of car id of roper silicon, and then heating the carbonaceous I than this; and the heating shoul be con-- tinued until the crust or layer of carbid of silicon has acquired a thickness corresponding to at least one-fourth the diameterof the core, and it is preferred to continue the heating until the crust-of carbid of silicon is nearly or quite one-half the diameter ofthe core.- Under these conditions only have I found it possible to establish and maintain a well-defined plane of demarcation between the finished separation o the carbid .of silicon from the outermost layers of graphite.

' I will describe the process. by 'reference'to tproducts and tosecure a clean.

the manufacture of a soft, unctuous and noncoalescing graphite suitable for lubricating purposes, it belng understood however that the. invention is-not limited to the manufacture of graphite of this particular grade, or to the manufacture of bulk graphite as distinguished from that of graphite articles.

T The furnace is provided with fixed terminals between. which extend one or more carbon or aphite; usually such bars 'or starting cores consisting of rods or bars of rods are. re atively short and a .number'of them are arranged in overlapping series or lon 'tudinal contact to estab 1sh the eas est patl i A single starting core may be employed, or two or more parallel coresmay be used, -these being surrounded by the. carbonai.

ceous material to be converted into'graphite. Such carbonaceous materlal may comprlse' petroleum coke suitably subdivided, oryanthracite' coal or other suitable form of car.-

bon, mixed if desired. with acertain proportion of silica or other materialcapable of-' ceous material'extends between the terminals forming a carbid. This, body of carbonaof the "furnace, and is completely'surrounded by a bed or envelop of sand and carbon in v roper proportions for theformation of .car-' v sufliciently porous to permit the-free escape of the reaction envelop of san id of silicon, and so constructed as to' be ases; Thethickfiess of this and carbon should bear a v certain'minimum roportion tothediamcter' of the bo dy of car on, and, as above pointed .of one-half the diameter of the core. "current is now turned on the furnace and gradually brought to the full load required out, it is found desirable in practice that the thickness of the envelop Should be in excess The for the graphitization of the carbon, but instead otceasin the passage of the current when the graphltization has been completed, or has proceeded to the extent of forming a commercial grade of graphite, the heating is continued, preferably but not necessarily at full load, until such time, as the mixture of sand and carbon, or the portion thereof adacent the graphite, is'converted into a firm,

coherent and non-friable mass or shell of 'carbid of silicon, whereof the constituent crystals are of such .character that they not only aggregate into a firm or coherent mass and exhibit but little tendency to become detached and commingled With'the graphite, but if so commingled are of such size.and shape as to be capable of complete separation by jigging or like simple process of concentration.

To obtain this result I have found itdesirable to continue the heating for to 36 hours or even longer, as distinguished from the, 12 to 18 hours usually practiced for graphitization. It will thus be period in excess of that r p associated with the carbon is volatilized with substantial completeness, and until the portion of the envelop adjacent'the carbonaceous mass is converted into a firm and coherent crystalline aggregate of carbid of silicon. r

The operation differs radically from that heretofore practiced in the manufacture of carbidof silicon in accordance with. my prior patents, Nos. 492,767 and 560,291, in

- that the-resistance core iscomposed of a material or charge adapted in its chemical charproduce acter, physical division and arrangement to raphite of commercial grade and high purity, and the heat is applied under proper conditions to effect such conversion.

In case articles of carbon are to be graphitized these are usually embedded in. a core material having a relatively low coeflicient of electrical conductivity, the arrangement being preferably substantially as described in my prior patent No. 702,7 58, granted June 17,- 1902.

From a purely technical or commercial point of view the present process is highly advantageous as compared either with the manufacture of graphite only or of carbid of silicon only. As compared 'with the 'rable from the manufacture of graphite it contemplates, it

is true,a greater expenditure of power, but

this is more than compensated by the/increased purity of the graphite, the increased yield from the furnace, .the saving oft me and expense in purification, and by the recovery of merchantable carbid of silicon as a by-product of the operation. As compared with the manufacture of carbid of silicon as heretofore practiced, it is highly'advantageous in that it yields in the zone of highest temperature a graphite. of marketable grade, instead of a corematerial which is adapted for useonly in a repetition of the process.

I claim: v

1. The method of making pure, unctuous graphite which consists in electrically heatmg a body or mass of carbonaceous material capable of transformation into such graphite, confining the heat therein and protecting the same from' oxidation by means of a permeable envelop completely surrounding the carbonaceous mass and containing sand and carbon in proper proportions to yield carbid of silicon, and continuing the heating until the carbonaceous material has been converted into an unctuous graphite of high purity, and a shell of carbid of silicon is formed surrounding .the graphite, the portion of the shell ad acent the graphite being constituted of a firm, coherent andwnongraphite which consists in electrically heat- 1 mg a body or mass of carbonaceous material capable of transformation into such graphite, confining the heat therein and protecting the same from oxidation by means of a permeable envelop completely surroundin the carbonaceous mass and containing sand and carb onin proper proportions to yield carbid of silicon, sald envelop having a thickness corresponding to at least one-half the diameter of the carbonaceous material, and con- 1 tinuing the heating until the carbonaceous material has been converted into an unctuous'graphite of high purity and a shell of carbid of silicon is formed extending outwardly from the carbonaceous body to at least one-fourth the diameter ofsaid body, the portion of the envelop adjacent the graphite bein constituted of a firm, cohercut and nonriable mass or aggregation of EDWARD 'GOODRICH ACHESONT Witnesses:

FRANK N. Con, 'Gnonen SHIPSTON.

graphite, substantially as de- Correction in Letters'Patenf No. 933,944.

It is herehy certified'that in Letter Patent No. 933.94L granted Septemberlel,

191m, npon the aphlication of Edward Goodrich Acheson, of Niagara Falls, Ontario,

Canada, for an improvement in Methods of Making Pure Unetuous Graphite, an

error appears in the printed specification requiring correction as follows:' Page 2,

- line 125, the word eonstru cted .should read constituted} and that the saidLetters 1 Patent should be read with this correction therein that the same may conform to the I, record of the case in the Patent Otfice.

Signed and sealed this 7th day of Dev-ember, A. D., 1909.

[we E. B. MOORE,

(Jam/m [resin M7 of Patents. 

